Micro- and mesoporous supports for CO2 methanation catalysts: a comparison between SBA-15, MCM-41 and USY zeolite

M.C. Bacariza, I. Graça, S.S. Bebiano, J. M. Lopes, C. Henriques

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Abstract

Mesoporous SBA-15 synthesized by two different methods and MCM-41 were used as supports for Ni and Ni-Ce catalysts applied in CO2 methanation reaction. The performances obtained for both materials were compared taking into account the differences in terms of textural properties, Ni species and reaction mechanism. Results were compared with the reported in the literature for a microporous USY zeolite. XRD, DRS UV–Vis, H2-TPR and TEM were used for the characterization of the samples. Catalytic tests were performed under the same conditions for all catalysts. Finally, FTIR Operando studies were carried out in order to establish differences from the mechanistically point of view as well as in terms of CO2 adsorption species for the different samples. Promising data was obtained with the Ni-based SBA-15 catalysts whatever the preparation method. Despite the greater Ni particles size, MCM-41 also reported interesting catalytic performances, so that presenting the highest TOF values among the catalysts studied. The good results obtained for the MCM-41 could be explained by the lower amount of non-reactive carbonyl species adsorbed on the Ni0 particles surface during the reaction as well as by the enhanced interaction between metal and support reflected in the calculated band gap values. All the results are comparable to the obtained using a HNaUSY zeolite with Si/Al = 2.8 as support. Cerium incorporation on Ni/mesoporous supports allowed enhancing the CO2 conversion, especially at lower temperatures, as already reported for the zeolite-based samples.
LanguageEnglish
Pages72-83
Number of pages12
JournalChemical Engineering Science
Volume175
Early online date18 Sep 2017
DOIs
Publication statusPublished - 16 Jan 2018

Fingerprint

Methanation
Zeolites
Multicarrier modulation
Catalyst supports
Catalysts
Cerium
Energy gap
Metals
Particle size
Transmission electron microscopy
Adsorption
SBA-15
MCM-41
Temperature

Keywords

  • SBA-15
  • MCM-41
  • zeolite
  • nickel
  • CO2 methanation
  • FTIR Operando

Cite this

Bacariza, M.C. ; Graça, I. ; Bebiano, S.S. ; Lopes, J. M. ; Henriques, C. / Micro- and mesoporous supports for CO2 methanation catalysts : a comparison between SBA-15, MCM-41 and USY zeolite. In: Chemical Engineering Science . 2018 ; Vol. 175. pp. 72-83.
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Micro- and mesoporous supports for CO2 methanation catalysts : a comparison between SBA-15, MCM-41 and USY zeolite. / Bacariza, M.C.; Graça, I.; Bebiano, S.S.; Lopes, J. M.; Henriques, C.

In: Chemical Engineering Science , Vol. 175, 16.01.2018, p. 72-83.

Research output: Contribution to journalArticle

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T1 - Micro- and mesoporous supports for CO2 methanation catalysts

T2 - Chemical Engineering Science

AU - Bacariza, M.C.

AU - Graça, I.

AU - Bebiano, S.S.

AU - Lopes, J. M.

AU - Henriques, C.

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N2 - Mesoporous SBA-15 synthesized by two different methods and MCM-41 were used as supports for Ni and Ni-Ce catalysts applied in CO2 methanation reaction. The performances obtained for both materials were compared taking into account the differences in terms of textural properties, Ni species and reaction mechanism. Results were compared with the reported in the literature for a microporous USY zeolite. XRD, DRS UV–Vis, H2-TPR and TEM were used for the characterization of the samples. Catalytic tests were performed under the same conditions for all catalysts. Finally, FTIR Operando studies were carried out in order to establish differences from the mechanistically point of view as well as in terms of CO2 adsorption species for the different samples. Promising data was obtained with the Ni-based SBA-15 catalysts whatever the preparation method. Despite the greater Ni particles size, MCM-41 also reported interesting catalytic performances, so that presenting the highest TOF values among the catalysts studied. The good results obtained for the MCM-41 could be explained by the lower amount of non-reactive carbonyl species adsorbed on the Ni0 particles surface during the reaction as well as by the enhanced interaction between metal and support reflected in the calculated band gap values. All the results are comparable to the obtained using a HNaUSY zeolite with Si/Al = 2.8 as support. Cerium incorporation on Ni/mesoporous supports allowed enhancing the CO2 conversion, especially at lower temperatures, as already reported for the zeolite-based samples.

AB - Mesoporous SBA-15 synthesized by two different methods and MCM-41 were used as supports for Ni and Ni-Ce catalysts applied in CO2 methanation reaction. The performances obtained for both materials were compared taking into account the differences in terms of textural properties, Ni species and reaction mechanism. Results were compared with the reported in the literature for a microporous USY zeolite. XRD, DRS UV–Vis, H2-TPR and TEM were used for the characterization of the samples. Catalytic tests were performed under the same conditions for all catalysts. Finally, FTIR Operando studies were carried out in order to establish differences from the mechanistically point of view as well as in terms of CO2 adsorption species for the different samples. Promising data was obtained with the Ni-based SBA-15 catalysts whatever the preparation method. Despite the greater Ni particles size, MCM-41 also reported interesting catalytic performances, so that presenting the highest TOF values among the catalysts studied. The good results obtained for the MCM-41 could be explained by the lower amount of non-reactive carbonyl species adsorbed on the Ni0 particles surface during the reaction as well as by the enhanced interaction between metal and support reflected in the calculated band gap values. All the results are comparable to the obtained using a HNaUSY zeolite with Si/Al = 2.8 as support. Cerium incorporation on Ni/mesoporous supports allowed enhancing the CO2 conversion, especially at lower temperatures, as already reported for the zeolite-based samples.

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